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Hydrodenitrogenation (HDN) is one of the most important catalytic hydrotreating reactions. Polycyclic nitrogen compounds that have a carbocycle and a five‐ or six‐membered heterocycle are the major nitrogen‐containing species in industrial feedstocks. In this review, thermodynamics, CN bond cleavage, HDN mechanisms of model compounds and reaction mixtures are discussed. Hydrotreating catalysts, kinetic modeling, and adsorption active sites are topics that are also covered.